Approach to hyperuniformity in a metallic glass-forming material exhibiting a fragile to strong glass transition

We investigate a metallic glass-forming (GF) material (Al₉₀Sm₁₀) exhibiting a fragile-strong (FS) glass-formation by molecular dynamics simulation to better understand this highly distinctive pattern of glass-formation in which many of the usual phenomenological relations describing relaxation times and diffusion of ordinary GF liquids no longer apply, and where instead genuine thermodynamic features are observed in response functions and little thermodynamic signature is exhibited at the glass transition temperature, T_g. Given the many unexpected similarities between the thermodynamics and dynamics of this metallic GF material with water, we first focus on the anomalous static scattering in this liquid, following recent studies on water, silicon and other FS GF liquids. We quantify the "hyperuniformity index" H of our liquid, which provides a quantitative measure of molecular "jamming". To gain insight into the T-dependence and magnitude of H, we also estimate another more familiar measure of particle localization, the Debye-Waller parameter 〈u²〉 describing the mean-square particle displacement on a timescale on the order of the fast relaxation time, and we also calculate H and 〈u²〉 for heated crystalline Cu. This comparative analysis between H and 〈u²〉 for crystalline and metallic glass materials allows us to understand the critical value of H on the order of 10^-3 as being analogous to the Lindemann criterion for both the melting of crystals and the "softening" of glasses. We further interpret the emergence of FS GF and liquid-liquid phase separation in this class of liquids to arise from a cooperative self-assembly process in the GF liquid.